Here, we confined fluorescent probes to solid nanochannels to construct nanosensors, which not only significantly improved the reusability of the molecular probes, but also achieved ion current and fluorescence dual gating for more reliable detection. The combination of optical and electrical modalities can provide comprehensive spatiotemporal information that can be used to elucidate the sensing mechanism within the nanochannel. As a proof-of-concept experiment, fluorescein isothiocyanate (FITC)–hydrazine (NH) was selected to modify nanochannels for the effective detection of Hg . Based on spirolactam opening tactics, the system synergistically alters the surface charge and fluorescence intensity in response to Hg, establishing a dual open state of current and fluorescence. The newly prepared nanosensor exhibited a fast response (<1 min), high sensitivity, and selectivity towards Hg . Importantly, the nanodevice could be recovered by simple NH treatment. Such sensing behavior could be used to implement optoelectronic dual-output XOR logical gates under the management of Hg and NH . This strategy is anticipated to find broad applications in other nanochannel-based systems for various sensing applications used for monitoring of pollutants, food additives, and biomolecules.